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Title: New insights into the design of conjugated polymers for intramolecular singlet fission

Abstract

Singlet fission (SF), a multiple exciton generation process which generates two triplet excitons after the absorption of one photon, can potentially enable more efficient solar cell designs, by harvesting energy normally lost as heat. While low-bandgap conjugated polymers are the highly promising candidates for efficient SF-based solar cells, few polymer materials capable of SF have been reported because the SF process in polymer chains is poorly understood. Using transient spectroscopy, we demonstrate a new, highly efficient (triplet yield of 160~200%) isoindigo-based donor-acceptor polymer and show that the triplet pairs are directly emissive and exhibit a time dependent energy evolution. Importantly, aggregation in poor solvents and in films significantly lowers the singlet energy, suppressing triplet formation because the energy conservation criterion is no longer met. These results suggest a new design rule for developing intramolecular SF capable low-bandgap conjugated polymers whereby inter-chain interactions must be carefully engineered.

Authors:
 [1];  [1];  [1]; ORCiD logo [2];  [1];  [3];  [4]; ORCiD logo [1]; ORCiD logo [5]
  1. Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing, School of Chemistry, Chemical Engineering and Life Science
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Peking Univ., Beijing (China). Beijing National Lab. for Molecular Sciences (BNLMS), Key Lab. of Bioorganic Chemistry and Molecular Engineering of Ministry of Education; Key Lab. of Polymer Chemistry and Physics of Ministry of Education; Center of Soft Matter Science and Engineering; College of Chemistry and Molecular Engineering
  4. Peking Univ., Beijing (China). Beijing National Lab. for Molecular Sciences (BNLMS), Key Lab. of Bioorganic Chemistry and Molecular Engineering of Ministry of Education; Key Lab. of Polymer Chemistry and Physics of Ministry of Education; Center of Soft Matter Science and Engineering; College of Chemistry and Molecular Engineering
  5. Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing, School of Chemistry, Chemical Engineering and Life Science; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC); Wuhan University of Technology
OSTI Identifier:
1474070
Report Number(s):
[BNL-209083-2018-JAAM]
[Journal ID: ISSN 2041-1723]
Grant/Contract Number:  
[SC0012704]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
[ Journal Volume: 9; Journal Issue: 1]; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 14 SOLAR ENERGY; 25 ENERGY STORAGE

Citation Formats

Hu, Jiahua, Xu, Ke, Shen, Lei, Wu, Qin, He, Guiying, Wang, Jie-Yu, Pei, Jian, Xia, Jianlong, and Sfeir, Matthew Y. New insights into the design of conjugated polymers for intramolecular singlet fission. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05389-w.
Hu, Jiahua, Xu, Ke, Shen, Lei, Wu, Qin, He, Guiying, Wang, Jie-Yu, Pei, Jian, Xia, Jianlong, & Sfeir, Matthew Y. New insights into the design of conjugated polymers for intramolecular singlet fission. United States. doi:10.1038/s41467-018-05389-w.
Hu, Jiahua, Xu, Ke, Shen, Lei, Wu, Qin, He, Guiying, Wang, Jie-Yu, Pei, Jian, Xia, Jianlong, and Sfeir, Matthew Y. Tue . "New insights into the design of conjugated polymers for intramolecular singlet fission". United States. doi:10.1038/s41467-018-05389-w. https://www.osti.gov/servlets/purl/1474070.
@article{osti_1474070,
title = {New insights into the design of conjugated polymers for intramolecular singlet fission},
author = {Hu, Jiahua and Xu, Ke and Shen, Lei and Wu, Qin and He, Guiying and Wang, Jie-Yu and Pei, Jian and Xia, Jianlong and Sfeir, Matthew Y.},
abstractNote = {Singlet fission (SF), a multiple exciton generation process which generates two triplet excitons after the absorption of one photon, can potentially enable more efficient solar cell designs, by harvesting energy normally lost as heat. While low-bandgap conjugated polymers are the highly promising candidates for efficient SF-based solar cells, few polymer materials capable of SF have been reported because the SF process in polymer chains is poorly understood. Using transient spectroscopy, we demonstrate a new, highly efficient (triplet yield of 160~200%) isoindigo-based donor-acceptor polymer and show that the triplet pairs are directly emissive and exhibit a time dependent energy evolution. Importantly, aggregation in poor solvents and in films significantly lowers the singlet energy, suppressing triplet formation because the energy conservation criterion is no longer met. These results suggest a new design rule for developing intramolecular SF capable low-bandgap conjugated polymers whereby inter-chain interactions must be carefully engineered.},
doi = {10.1038/s41467-018-05389-w},
journal = {Nature Communications},
number = [1],
volume = [9],
place = {United States},
year = {2018},
month = {7}
}

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    Works referencing / citing this record:

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